CN110010205A - A method of assessment self-catalysis substance thermal stability - Google Patents
A method of assessment self-catalysis substance thermal stability Download PDFInfo
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- CN110010205A CN110010205A CN201910215624.8A CN201910215624A CN110010205A CN 110010205 A CN110010205 A CN 110010205A CN 201910215624 A CN201910215624 A CN 201910215624A CN 110010205 A CN110010205 A CN 110010205A
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Abstract
The invention belongs to the thermally safe field of chemical process, especially a kind of method for assessing self-catalysis substance thermal stability.The following steps are included: step 1: being analyzed based on self-catalysis Proto models fitting；Step 2: self-catalysis TMRadThe it is proposed of analytic formula；Self-catalysis Proto model and N grades of models are compared, the TMR based on Proto model is proposed according to comparison resultadAnalytic formula；Step 3: numerical value, which calculates, determines undetermined coefficient X；Step 4: analytic formula calculates TMRadObtain thermal stability evaluation result；Undetermined coefficient is determined by the parameter of Fitting Analysis, and by its back substitution to TMRadIt is calculated in analytic formula obtained from catalysis TMRadAssessment result obtains thermal stability evaluation result.A kind of method for assessment self-catalysis substance thermal stability that the application proposes, the self-catalysis substance TMR of assessmentadIt is more accurate compared to existing calculation method calculated result reliable.
Description
Technical field
The invention belongs to the thermally safe field of chemical process, especially a kind of method for assessing self-catalysis substance thermal stability.
Background technique
Under the overall background that chemical industry rapidly develops, people gradually recognize the risk of chemical heat release and gradually
Form the reaction heat safety evaluation method of the system cognizant and more system to this kind of reaction thermal hazard.
Maximum reaction rate arrival time (Time to maximum rate under adiabatic under adiabatic condition
condition, TMRad) it is widely applied parameter in substance thermal stability and the thermally safe assessment of chemical process, principle is can
For taking the time of safeguard measure longer, a possibility that runaway reaction occurs lower, the arrival maximum that is derived reaction
Initial decomposition temperature T when the time of rate is for 24 hoursD24It is also the Common Concepts that technological temperature is determined in production process.
TMRadIt is proposed earliest by Semenoff, Townsend and Tou are successfully developing acceleration adiabatic calorimetry instrument
On the basis of (Accelerating Rate Calorimeter, ARC), referred to during analyzing experimental data
The concept, and TMR is proposed based on N grades of modelsadIntegral formulas and the analytical expression that generally uses now, then should
Method is widely accepted and becomes the TMR of many commercial adiabatic calorimetry equipment defaultsadAcquiring method.In addition, N grades of models are based on,
Townsend has been derived by ln (TMRad) with the linear relationship of 1/T, this is also TMRadAnd TD24Calculating provide easy meter
The thinking of calculation: ln (TMR is utilizedad) with the linear relationship of 1/T, be extrapolated to the T that can be obtained substance under cryogenic conditionsD24, that is, extrapolate
Method.
The above two TMR based on N grades of modelsadCalculation method be the Material Thermal Stability Evaluation generallyd use in engineering and
Process heat safety evaluation method has many advantages, such as easy, quick.But it is very complicated in real reaction process, N grades of models are past
Toward being not enough to describe different types of reaction process, especially for this substance of self-catalysis, based on N grades of TMRadAssessment can
There can be deviation even complete mistake.
Summary of the invention
Technical problem solved by the invention is to provide a kind of method for assessing self-catalysis substance thermal stability, to improve
The unicity and limitation of existing appraisal procedure provide new solution for the engineering simplification of self-catalysis Material Thermal Stability Evaluation
Thinking.
The technical solution for realizing the aim of the invention is as follows:
A method of assessment self-catalysis substance thermal stability, comprising the following steps:
Step 1: it is analyzed based on self-catalysis Proto models fitting；Using self-catalysis Proto model to self-catalysis substance
Measured data carries out dynamic analysis and obtains kinetic parameter；
Step 2: self-catalysis TMRadThe it is proposed of analytic formula；Self-catalysis Proto model and N grades of models are compared, root
The TMR based on Proto model is proposed according to comparison resultadAnalytic formula；
Step 3: numerical value, which calculates, determines undetermined coefficient X；Influence by each parameter of numerical Analysis to undetermined coefficient,
According to substance decomposition dynamics statistical result, suitable analyst coverage is taken on the parameter for significantly affecting undetermined coefficient, that is, takes insulation
20-100 DEG C of temperature rise, order of reaction 0-1, pass through the undetermined coefficient under numerical simulation calculation different parameters value；
Step 4: analytic formula calculates TMRadObtain thermal stability evaluation result；It is determined by the parameter of Fitting Analysis undetermined
Coefficient, and by its back substitution to TMRadIt is calculated in analytic formula obtained from catalysis TMRadAssessment result obtains thermal stability evaluation knot
Fruit.
Further, self-catalysis TMR described in the step 2adThe it is proposed of analytic formula, specific as follows:
By self-catalysis Proto model compared with N grades of models carry out analysis, analytic process is as follows:
N grades of models of single step:
In formula, (dT/dt)_nFor the temperature rise rate equation of N grades of models of single step, DEG C；A is pre-exponential factor, s-1；EaFor reaction
Apparent activation energy, kJmol-1；N is the order of reaction；R is gas constant, 8.314JK-1·mol-1；ΔTadFor adiabatic temperature rise,
That is Tf-T0, DEG C；TfFor heat release final temperature, DEG C；T is the temperature under any time, DEG C；TmIt is corresponding for temperature rise rate maximum
Temperature, DEG C；mmFor temperature rise rate maximum value, DEG C min-1；TMRad_nFor the maximum reaction rate arrival time of N grades of models of single step
Integral formula；
Self-catalysis Proto model:
In formula, (dT/dt)_aFor the temperature rise rate equation of self-catalysis Proto model, DEG C；n1And n2For the order of reaction；
TMRad_aFor the maximum reaction rate arrival time integral formula of self-catalysis Proto model；
Above-mentioned temperature rise rate equation and TMR for single step N grades of model and self-catalysis Proto modeladIntegral calculation equation,
By comparing it is found that the temperature rise rate of self-catalysis Proto model only has more compared to N grades of models of single stepThis
, and T0≤T≤Tf,ThereforeThen self-catalysis
The TMR of Proto modeladAlso approximate to pass through the TMR of N grades of model inferences of single stepadIt is indicated:
In formula, corresponding temperature is not maximum reaction rate under N grades of models of single step at maximum temperature rise rate under Proto model
Locate corresponding temperature, but since quickly, the time difference for reaching the two temperature is negligible, therefore still may be used for reaction rate under high temperature
Think that above formula is set up, it may be assumed that TMRad_a>TMRad_n2；
Thus, it is supposed that there are some undetermined coefficient X (0 < X < 1), so thatIt sets up, then self-catalysis
The TMR of Proto modeladAnalytic formula is are as follows:
Further, numerical value described in the step 3, which calculates, determines undetermined coefficient X, specific as follows:
Using numerical computation method analysis undetermined coefficient to the sensitivity to parameter of each kinetic parameter, and on significantly affect to
The kinetic parameter for determining coefficient value takes suitable analysis range, that is, takes 20-100 DEG C of adiabatic temperature rise, order of reaction 0-1, using base
The undetermined coefficient obtained under different parameters value is calculated in the numerical computation method of four step Runge-Kutta.
Compared with prior art, the present invention its remarkable advantage:
(1) method for a kind of assessment self-catalysis substance thermal stability that the application proposes, the self-catalysis substance TMR of assessmentad
It is more accurate compared to existing calculation method calculated result reliable；
(2) the method calculating process for the assessment self-catalysis substance thermal stability that the application proposes is convenient, is convenient for self-catalysis object
The engineering simplification application of matter thermal stability.
Present invention is further described in detail with reference to the accompanying drawing.
Detailed description of the invention
Fig. 1 is self-catalysis Material Thermal Stability Evaluation process in the present invention.
Fig. 2 is the tool that the numerical computation method iteration based on four step Runge-Kutta seeks undetermined coefficient X in the present invention
Body calculation flow chart.
Fig. 3 is that cumyl hydroperoxide measured curve is quasi- using single step N grades and self-catalysis Proto model analysis in the present invention
It closes as a result, wherein figure (a) is temperature-time curve, figure (b) is temperature rise rate-time graph.
Fig. 4 is adiabatic temperature rise Δ T different under self-catalysis Proto model in the present inventionadWith differential responses series n1Lower correspondence
Undetermined coefficient X.
Fig. 5 is the self-catalysis TMR of cumyl hydroperoxide in the present inventionadAnalytic formula calculated result and be based on Proto mould
The TMR of type analysis assessmentadAs a result.
Specific embodiment
As shown in Figure 1, the present invention proposes a kind of method for assessing self-catalysis substance thermal stability, which includes step 1
~4, the present invention is described in further detail below in conjunction with the accompanying drawings:
Step 1: it is analyzed based on self-catalysis Proto models fitting；Using self-catalysis Proto model to self-catalysis substance
Measured data carries out dynamic analysis and obtains kinetic parameter；Here N grades of models of self-catalysis Proto model and single step are respectively adopted
The measured curve of cumyl hydroperoxide is fitted, fitting effect is as shown in figure 3, the resulting kinetic parameter of Fitting Analysis
It is shown in Table 1.It can be seen from the figure that the fitting effect under two kinds of kinetic models is all fine, this meaning using single ARC curve into
Action mechanics easily causes error when asking calculation.
The kinetic parameter (N grades of models of Proto model and single step) that the fitting of table 1 obtains
Step 2: self-catalysis TMRadThe it is proposed of analytic formula；Self-catalysis Proto model and N grades of models are subjected to analysis ratio
Compared with according to the TMR of comparison result proposition based on this modeladAnalytic formula；Self-catalysis Proto model and N grades of models are divided
Analysis is compared, and analytic process is as follows:
N grades of models of single step:
In formula, (dT/dt)_nFor the temperature rise rate equation of N grades of models of single step, DEG C；A is pre-exponential factor, s-1；EaFor reaction
Apparent activation energy, kJmol-1；N is the order of reaction；R is gas constant, 8.314JK-1·mol-1；ΔTadFor adiabatic temperature rise,
That is Tf-T0, DEG C；TfFor heat release final temperature, DEG C；T is the temperature under any time, DEG C；TmIt is corresponding for temperature rise rate maximum
Temperature, DEG C；mmFor temperature rise rate maximum value, DEG C min-1；TMRad_nFor the maximum reaction rate arrival time of N grades of models of single step
Integral formula.
Self-catalysis Proto model:
In formula, (dT/dt)_aFor the temperature rise rate equation of self-catalysis Proto model, DEG C；n1And n2For the order of reaction；
TMRad_aFor the maximum reaction rate arrival time integral formula of self-catalysis Proto model.
Above-mentioned temperature rise rate equation and TMR for single step N grades of model and self-catalysis Proto modeladIntegral calculation equation.
By comparing it is found that the temperature rise rate of self-catalysis Proto model only has more compared to N grades of models of single stepThis
, and T0≤T≤Tf,ThereforeThen self-catalysis
The TMR of Proto modeladAlso approximate to pass through the TMR of N grades of model inferences of single stepadIt is indicated:
In formula, corresponding temperature is not maximum reaction rate under N grades of models of single step at maximum temperature rise rate under Proto model
Locate corresponding temperature, but since quickly, the time difference for reaching the two temperature is negligible, therefore still may be used for reaction rate under high temperature
Think that above formula is set up, it may be assumed that TMRad_a>TMRad_n2。
Thus, it is supposed that there are some undetermined coefficient X (0 < X < 1), so thatIt sets up, then self-catalysis
The TMR of Proto modeladAnalytic formula is are as follows:
Step 3: numerical value, which calculates, determines undetermined coefficient X, the influence by each parameter of numerical Analysis to undetermined coefficient,
According to substance decomposition dynamics statistical result, suitable analyst coverage is taken on the parameter for significantly affecting undetermined coefficient, that is, takes temperature rise
Rate passes through the undetermined coefficient under numerical simulation calculation different parameters value；It is specific as follows:
According to substance decomposition dynamics statistical result, zone of reasonableness is taken to each kinetic parameter involved in model, is such as referred to
Prefactor 102-1020s-1；Activation energy 50-250kJmol-1；Order of reaction 1-3 etc..It is analyzed using numerical computation method undetermined
Coefficient finds the sensitivity to parameter of each parameter by a large amount of numerical analysis, in self-catalysis Proto model, order of reaction
Number n1And adiabatic temperature rise Δ TadVery big on the influence of the value of undetermined coefficient X, influence of other kinetic parameters to X be not significant.
Therefore the analyst coverage of the suitable order of reaction and adiabatic temperature rise, i.e. 0 < n are taken1< 1,20≤Δ Tad≤ 100, using based on quadravalence
The numerical Analysis of Runge-Kutta method obtains the undetermined coefficient under different dynamic parameter value, analyzes numerical value used
Calculation method calculation process is shown in Fig. 2, and corresponding undetermined coefficient X calculated result is as shown in Figure 4 under each parameter value.
Step 4: analytic formula calculates TMRad；Undetermined coefficient is determined by the parameter of Fitting Analysis, and its back substitution is arrived
TMRadIt is calculated in analytic formula obtained from catalysis TMRadAssessment result obtains thermal stability evaluation result.
Step 4: analytic formula calculates TMRadObtain thermal stability evaluation result；By the kinetic parameter analyzed determine to
Coefficient is determined, by its back substitution to TMRadIt is calculated in analytic formula and obtains TMR under Proto modeladAssessment result；It is specific as follows:
According to the kinetic parameter that 1 Fitting Analysis of table obtains, it is 0.55 that undetermined coefficient X is read from Fig. 4, is substituted into formula
(1) self-catalysis substance TMR is carried outadAnalytic formula calculates, with the TMR under Proto modeladAssessment result is compared such as Fig. 5 institute
Show, the T that analytic formula calculatesD24It is 84.15 DEG C, the T based on self-catalysis Proto model analysisD24It is 85.21 DEG C, the two analysis
As a result deviation is little between, and analytic formula calculated result is more reliable.
Claims (3)
1. a kind of method for assessing self-catalysis substance thermal stability, which comprises the following steps:
Step 1: it is analyzed based on self-catalysis Proto models fitting；Actual measurement using self-catalysis Proto model to self-catalysis substance
Data carry out dynamic analysis and obtain kinetic parameter；
Step 2: self-catalysis TMRadThe it is proposed of analytic formula；Self-catalysis Proto model and N grades of models are compared, according to than
Relatively result proposes the TMR based on Proto modeladAnalytic formula；
Step 3: numerical value, which calculates, determines undetermined coefficient X；Influence by each parameter of numerical Analysis to undetermined coefficient, according to
Substance decomposition dynamics statistical result takes suitable analyst coverage to the parameter for significantly affecting undetermined coefficient, that is, takes adiabatic temperature rise
20-100 DEG C, order of reaction 0-1, pass through the undetermined coefficient under numerical simulation calculation different parameters value；
Step 4: analytic formula calculates TMRadObtain thermal stability evaluation result；Undetermined coefficient is determined by the parameter of Fitting Analysis,
And by its back substitution to TMRadIt is calculated in analytic formula obtained from catalysis TMRadAssessment result obtains thermal stability evaluation result.
2. a kind of method for assessing self-catalysis substance thermal stability according to claim 1, which is characterized in that the step
Self-catalysis TMR described in twoadThe it is proposed of analytic formula, specific as follows:
By self-catalysis Proto model compared with N grades of models carry out analysis, analytic process is as follows:
N grades of models of single step:
In formula, (dT/dt)_nFor the temperature rise rate equation of N grades of models of single step, DEG C；A is pre-exponential factor, s-1；EaFor the apparent of reaction
Activation energy, kJmol-1；N is the order of reaction；R is gas constant, 8.314JK-1·mol-1；ΔTadFor adiabatic temperature rise, i.e.,
Tf-T0, DEG C；TfFor heat release final temperature, DEG C；T is the temperature under any time, DEG C；TmFor the corresponding temperature of temperature rise rate maximum
Degree, DEG C；mmFor temperature rise rate maximum value, DEG C min-1；TMRad_nFor the product of maximum reaction rate arrival time of N grades of models of single step
Divide formula；
Self-catalysis Proto model:
In formula, (dT/dt)_aFor the temperature rise rate equation of self-catalysis Proto model, DEG C；n1And n2For the order of reaction；TMRad_aFor
The maximum reaction rate arrival time integral formula of self-catalysis Proto model；
Above-mentioned temperature rise rate equation and TMR for single step N grades of model and self-catalysis Proto modeladIntegral calculation equation, pass through
Comparison is it is found that the temperature rise rate of self-catalysis Proto model only has more compared to N grades of models of single stepThis, and
T0≤T≤Tf,ThereforeThen self-catalysis Proto model
TMRadAlso approximate to pass through the TMR of N grades of model inferences of single stepadIt is indicated:
In formula, corresponding temperature is not under N grades of models of single step at maximum reaction rate pair at maximum temperature rise rate under Proto model
The temperature answered, but since quickly, the time difference for reaching the two temperature is negligible, therefore is still believed that for reaction rate under high temperature
Above formula is set up, it may be assumed that TMRad_a> TMRad_n2；
Thus, it is supposed that there are some undetermined coefficient X (0 < X < 1), so thatIt sets up, then self-catalysis Proto mould
The TMR of typeadAnalytic formula is are as follows:
3. a kind of method for assessing self-catalysis substance thermal stability according to claim 1, which is characterized in that the step
Numerical value described in three, which calculates, determines undetermined coefficient X, specific as follows:
Using numerical computation method analysis undetermined coefficient to the sensitivity to parameter of each kinetic parameter, and on significantly affecting system undetermined
The kinetic parameter of number value takes suitable analysis range, that is, takes 20-100 DEG C of adiabatic temperature rise, order of reaction 0-1, using based on four
The numerical computation method of rank Runge-Kutta method calculates the undetermined coefficient obtained under different parameters value.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112033997A (en) * | 2020-08-17 | 2020-12-04 | 西安近代化学研究所 | Explosive thermal stability grading method based on differential scanning calorimetry |
| CN112033998A (en) * | 2020-08-17 | 2020-12-04 | 西安近代化学研究所 | Thermal insulation acceleration calorimetry-based explosive material thermal stability grading method |
| CN112102892A (en) * | 2020-08-17 | 2020-12-18 | 西安近代化学研究所 | Method for determining temperature correction coefficient of energetic material chemical combination process |
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2019
- 2019-03-21 CN CN201910215624.8A patent/CN110010205A/en not_active Withdrawn
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112033997A (en) * | 2020-08-17 | 2020-12-04 | 西安近代化学研究所 | Explosive thermal stability grading method based on differential scanning calorimetry |
| CN112033998A (en) * | 2020-08-17 | 2020-12-04 | 西安近代化学研究所 | Thermal insulation acceleration calorimetry-based explosive material thermal stability grading method |
| CN112102892A (en) * | 2020-08-17 | 2020-12-18 | 西安近代化学研究所 | Method for determining temperature correction coefficient of energetic material chemical combination process |
| CN112033997B (en) * | 2020-08-17 | 2023-02-14 | 西安近代化学研究所 | Explosive thermal stability grading method based on differential scanning calorimetry |
| CN112102892B (en) * | 2020-08-17 | 2023-05-09 | 西安近代化学研究所 | Method for determining temperature correction coefficient of energetic material combination process |
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Application publication date: 20190712 |